Hydrogenation of iron nanoparticles was performed both computationally and experimentally where previously chemically-bonded iron hydride is considered to be unachievable under ordinary conditions. Density functional theory (DFT) calculations predict that hydrogenated iron nanoparticles are stabilized on a single-layer graphene/Cu substrate. Experimentally, iron nanoparticles were deposited onto a graphene/Cu substrate by vacuum deposition. Hydrogenation was done at 1atm of hydrogen gas and under liquid nitrogen. Mass spectrometry peak confirmed the hydrogen release from hydrogenated iron nanoparticles while a scanning transmission electron microscopy is used in order to link a geometrical shape of iron hydride nanoparticles between experimental and theoretical treatments. The hydrogenated iron nanoparticles were successfully synthesized where hydrogenated iron nanoparticles are stable under ordinary conditions.